James C. Greer

Silicon nanowire band gap modification.

Band gap modification for small-diameter (approximately 1 nm) silicon nanowires resulting from the use of different species for surface termination is investigated by density functional theory calculations. Because of quantum confinement, small-diameter wires exhibit a direct band gap that increases as the wire diameter narrows, irrespective of surface termination. This effect has been observed in previous experimental and theoretical studies for hydrogenated wires. For a fixed cross-section, the functional group used to saturate the silicon surface significantly modifies the band gap, resulting in relative energy shifts of up to an electronvolt. The band gap shifts are traced to details of the hybridization between the silicon valence band and the frontier orbitals of the terminating group, which is in competition with quantum confinement.

Simulation of junctionless Si nanowire transistors with 3 nm gate length

Inspired by recent experimental realizations and theoretical simulations of thin silicon nanowire-based devices, we perform proof-of-concept simulations of junctionless gated Si nanowire transistors. Based on first-principles, our primary predictions are that Si-based transistors are physically possible without major changes in design philosophy at scales of ∼1 nm wire diameter and ∼3 nm gate length, and that the junctionless transistor avoids potentially serious difficulties affecting junctioned channels at these length scales. We also present investigations into atomic-level design factors such as dopant positioning and concentration.Inspired by recent experimental realizations and theoretical simulations of thin silicon nanowirebased devices, we perform predictive first-principles simulations of junctionless gated Si nanowire transistors. Our primary predictions are that Si-based transistors are physically possible without major changes in design philosophy at scales of ∼1 nm wire diameter and ∼3 nm gate length, and that the junctionless transistor [1, 2] may be the only physically sensible design at these length scales. We also present investigations into atomic-level design factors such as dopant positioning and concentration.

Ballistic conductance in oxidized Si nanowires.

The influence of local oxidation in silicon nanowires on hole transport, and hence the effect of varying the oxidation state of silicon atoms at the wire surface, is studied using density functional theory in conjunction with a Greens function scattering method. For silicon nanowires with growth direction along [110] and diameters of a few nanometers, it is found that the introduction of oxygen bridging and back bonds does not significantly degrade hole transport for voltages up to several hundred millivolts relative to the valence band edge. As a result, the mean free paths are comparable to or longer than the wire lengths envisioned for transistor and other nanoelectronics applications. Transport along [100]-oriented nanowires is less favorable, thus providing an advantage in terms of hole mobilities for [110] nanowire orientations, as preferentially produced in some growth methods.

Monte Carlo configuration interaction predictions for the electronic spectra of Ne, CH2, C2, N2, and H2O compared to full configuration interaction calculations.

Singlet and triplet electronic excitation energies have been calculated for Ne, CH(2), C(2), N(2), and H(2)O using the Monte Carlo configuration interaction (CI) method. We find that excitation energies can be predicted to within a few tens of meV of full CI (FCI) results using expansions consisting of only a few thousand configuration state functions as compared to the O(10(8)) configurations occurring in the corresponding FCI expansions. The method provides a consistently accurate and balanced description of electronic excitations with accuracy for small molecular systems comparable to the equation-of-motion coupled cluster method with full triples.

A proposed confinement modulated gap nanowire transistor based on a metal (tin).

Energy bandgaps are observed to increase with decreasing diameter due to quantum confinement in quasi-one-dimensional semiconductor nanostructures or nanowires. A similar effect is observed in semimetal nanowires for sufficiently small wire diameters: A bandgap is induced, and the semimetal nanowire becomes a semiconductor. We demonstrate that on the length scale on which the semimetal-semiconductor transition occurs, this enables the use of bandgap engineering to form a field-effect transistor near atomic dimensions and eliminates the need for doping in the transistors source, channel, or drain. By removing the requirement to supply free carriers by introducing dopant impurities, quantum confinement allows for a materials engineering to overcome the primary obstacle to fabricating sub-5 nm transistors, enabling aggressive scaling to near atomic limits.

Tunnelling in alkanes anchored to gold electrodes via amine end groups.

For investigation of electron transport on the nanoscale, a system possessing a simple-to-interpret electronic structure is composed of alkane chains bridging two electrodes via end groups; to date, the majority of experiments and theoretical investigations on such structures have considered thiols bonding to gold electrodes. Recently experiments show that well-defined molecular conductances may be resolved if the thiol end groups are replaced by amines. In this theoretical study, we investigate the bonding of amine groups to gold clusters and calculate electron transport across the resulting tunnel junctions. We find very good agreement with recent experiments for alkane diamines and discuss differences with respect to the alkane dithiol system.

Spin-Polarization Mechanisms of the Nitrogen-Vacancy Center in Diamond

The nitrogen-vacancy (NV) center in diamond has shown great promise for quantum information due to the ease of initializing the qubit and of reading out its state. Here we show the leading mechanism for these effects gives results opposite from experiment; instead both must rely on new physics. Furthermore, NV centers fabricated in nanometer-sized diamond clusters are stable, motivating a bottom-up qubit approach, with the possibility of quite different optical properties to bulk.

A Monte Carlo configuration generation computer program for the calculation of electronic states of atoms, molecules, and quantum dots

The program mcci (Monte Carlo configuration interaction) is a simple to use and efficient means for performing configuration interaction (CI) calculations. As with all forms of CI, the basic problem is how to select new configurations for the expansion of the wavefunction and this is the issue addressed by mcci. The mcci program selects configurations through a Monte Carlo generation procedure and then iteratively refines the wavefunction. As a consequence, a compact CI vector results as opposed to traditional approaches such as excitation truncation. The program has been applied to the study of the ground state correlation energy of small molecules, to molecular dissociation problems, and to the calculation of the excited state spectra of atoms. The code performs well on single workstations or PCs and its use on parallel computers is discussed.

Nanoscale dynamics and protein adhesivity of alkylamine self-assembled monolayers on graphene.

Atomic-scale molecular dynamics computer simulations are used to probe the structure, dynamics, and energetics of alkylamine self-assembled monolayer (SAM) films on graphene and to model the formation of molecular bilayers and protein complexes on the films. Routes toward the development and exploitation of functionalized graphene structures are detailed here, and we show that the SAM architecture can be tailored for use in emerging applications (e.g., electrically stimulated nerve fiber growth via the targeted binding of specific cell surface peptide sequences on the functionalized graphene scaffold). The simulations quantify the changes in film physisorption on graphene and the alkyl chain packing efficiency as the film surface is made more polar by changing the terminal groups from methyl (-CH3) to amine (-NH2) to hydroxyl (-OH). The mode of molecule packing dictates the orientation and spacing between terminal groups on the surface of the SAM, which determines the way in which successive layers build up on the surface, whether via the formation of bilayers of the molecule or the immobilization of other (macro)molecules (e.g., proteins) on the SAM. The simulations show the formation of ordered, stable assemblies of monolayers and bilayers of decylamine-based molecules on graphene. These films can serve as protein adsorption platforms, with a hydrophobin protein showing strong and selective adsorption by binding via its hydrophobic patch to methyl-terminated films and binding to amine-terminated films using its more hydrophilic surface regions. Design rules obtained from modeling the atomic-scale structure of the films and interfaces may provide input into experiments for the rational design of assemblies in which the electronic, physicochemical, and mechanical properties of the substrate, film, and protein layer can be tuned to provide the desired functionality.

Determination of complex absorbing potentials from the electron self-energy

The electronic conductance of a molecule making contact to electrodes is determined by the coupling of discrete molecular states to the continuum electrode density of states. Interactions between bound states and continua can be modeled exactly by using the (energy-dependent) self-energy or approximately by using a complex potential. We discuss the relation between the two approaches and give a prescription for using the self-energy to construct an energy-independent, nonlocal, complex potential. We apply our scheme to studying single-electron transmission in an atomic chain, obtaining excellent agreement with the exact result. Our approach allows us to treat electron-reservoir couplings independent of single-electron energies, allowing for the definition of a one-body operator suitable for inclusion into correlated electron transport calculations.